Apparatus for manufacture of hydrogen and carbon-black.



R. H. BROWNLEE & R. H. UHLINGER.

APPARATUS FOR MANUFACTURE OF HYDROGEN AND CARBON BLACK.

APPLICATION FILED JAN. 15. I916.

Patented May 7,1918.

SHEET 1- 2 SHEETS- R. H. BROWNLEE (Y: R. H. UHLINGER.

APPARATUS FOR MANUFACTURE OF HYDROGEN AND CARBON BLACK.

APPLICATION EILED ml. 15. 1916.

Patented May 7,1918.

2 SHEETS-SHEET 2.

mounted adj ustably within the casing, as by hinged mountings 23. adapted to be raised to horizontal operative position as shown, or to be lowered, as indicated in dotted lines, whereby, by a suitable lever mechanism on the outside of the casing, any collected carbon may be dropped into the hopper below. The outlet at the upper portion of the casing is provided with a suitable safety valve 24 and a pressure indicating gage 25;

Beyond the screens is a conduit 31 leading to a water seal vessel 32, in which the terminal of the conduit is submerged and conduit 33 leads from the upper portion of water seal vessel 32 to a scrubber 34 of any suitable construction, provided with porous material 35, such as coke, and a water spray 36, whereby, by means of water, the gases.

are cooled and washed. Z

An additional scrubber 37 may also be provided, connected with the primary scrubber 34 by a circulation pipe 38, into which scrubber a spray pipe 39 of lime water or other alkaline material may be introduced, by which impurities in the hydrogen are removed, such as traces of sulfur compounds in the gas or other hydrocarbon used, the

'. hydrogen passing off by outlet pipe 40 to any suitable collectingor storage tank.

At any suitable point beyond the carbon separator or screen box 21 is the automatically regulated pressure relief valve 46 for holding the desired pressure in the furnace and carbon separator and the water seal 32,.

but may also be inserted in the line beyond the scrubbers, if preferred, for the same purpose.

It will also be understood that the pressure in the furnace 2 may be regulated by valve 15, or lower pressures may be regulated by the depth of the end of the conduit 31 in the water seal 32. Further when it is not remove these impurities, or any other suitable method of purification may be resorted to, as required.

Fig. 2 shows a modified arrangement of the furnace 2 whereby the heat of the refractory material leads downwardly from the top to a suitable outlet 6*, gas being furnished by pipe 12 having a valve 13 and air by pipe 10* having a valve 11.

The gas to be decomposed in such case enters through the base of the furnace by pipe 8, passing upwardly through the checkerwork 5 and outwardly at the top through conduit 14.

Said conduit is likewise provided with a controlling valve 15 and a conduit 16 extends vertically down within and through a body of. water 17 in casing 18 provided with a supply connection 19 and an overflow 20 I The lower end of the conduit opens into a hopper 21 of the same construction as above described, adapted to collect the carbon, the hydrogen passing off in the same manner and through the same apparatus, similarly indicated by numerals having the exponent a.

This arrangement and the operation carried out with the apparatus of Fig. 2 is desirable when hydrogen is the product required, as this procedure of passing the hydrocarbon upwardly under pressure decreases the amount of carbon which is carried over into the conveying conduit, and leaves more in the checkerwork where it is burned during the succeeding heating periods.

Fig. 3 shows a suitable apparatus for carrying out the method with a further or supplemental purification of the hydrogen when it contains carbon monoxid, as is ordinarily the case.

In such arrangement a furnace 2 similar in construction to the furnaces above described having the refractory material or metallic oxids 5 is adapted to receive the hydrogen coming over by pipe 40 having a suitable controlling valve 40, from the last scrubber 37, or directly from pipe 33.

Said conduit connects with a conduit 41' opening into the chamber 9 below supporting checkerwork 4", and into such conduit 41 is introduced a steam pipe 42 having a controllin valve 43 for the addition of steam.

Incidentally, a gas pipe 12 having a controlling valve 13, is introduced into conduit 41, and said conduit is provided with an extension 10 having a valve 11 for inlet of air, whereby to provide for the introduction of fuel and air for the pro-heating of the refractory material, the products of combustion the damper By this means, upon closing circulation of the gases through valve 40" and steam through pipe 42, the checkerwork 5 may be re-heated at the same time as the checker- I work 5 in the being heated.

, From such supplemental furnace 2 the gases after passing through the refractory primary furnace 2 or 2 is material are led off by conduit 44 having a I controlling valve 45, and if desired, a check valve 46", whereby the hydrogen and carbon dioxid are introduced into the base of a cooling tower 47.

passing off by stack 6 having 3 terial 35 and a water spray pipe 36, a conduit 38 leading the gases to one or more additional similar towers, similarly provided with porous material and spray 39 for introducing lime water or other alkaline material for the removal of the carbon dioxid. roduced in the furnace. The gas passing 9 rom the last scrubber by conduit 40 will be i very pure hydrogen if gas or bil free from nitrogen is originally used. I i The several scrubbers are provided at the bottom with discharge pipes for carrying 0d .the waste water and impurities.

It will be understood that it is essential to the operation that no oxidizable metals or easily reducible metallic oxids be contained in the lining or checkerwork of the furnace,

as in the first place, the refractory materials 'willl begreatly impaired, as is well-known;

and in t e second place, during the-heating upmperiod, metals, such .ascopper, iron, etc,

till

" 16 closed, gas (natural gas, coal'gas, oil vapor or other hydrocarbon, preferably as a j gas liquid or volatilizable solid), is admit .ted throughpipe .12 with a suitable amount I 5 the fuel.

be oxidized, as shown by the following familiar equations: I I Cu+O=1Cu0 3Fe+40=re,o, Then, during the production of hydrogen and carbon these oxids will be reduced to reform the metal and carbon 'monoxid. This is a fact ot' elementary chemistry.

' CuU-l-ll-L:Cu-i-ll-LJUP CuO-i-C=Cu+C In case hydrogen reduces the copperioxid and also to form copper and water, the latter will in turnbe reduced by the incandescent carbon in the furnace, so that the final result of the use of such is necessarily the addition of car- 'bo'n monoxid as an impurity to the hydrogen.

The greater the amount of metals or'metallic oxids present, the greater will be the proportion of carbon monoxid introduced. The operation of making hydrogen and carbon black, utilizing the aboye described apparatus, is as follows, havin'g reference to the apparatus of Fig. 1.

With the-valve 7 in stack 6 opened, and valve 1 15 to the carbon precipitating conduit of air by conduit 10 to chamber 9 below the checkerwork for the complete combustion of The products of combustion "pass up-.-'

wardly through'the interior of furnace 2 and its refractory contents 5, the operation being continued until the furnace and its contents 1 are heatedto a veryhigh temperature, a. a, above the'temperature' at which the hydrocarbons to be used in the formation of hydrogen andcarbon black are decomposed.

on a suitable temperature has thus been reached, say 1400 (3., or higheiythe air su ply and then the, as supply is shut 0d; t I

stack valve 7 is c osed, valve 15 to the carbon precipitator is opened, and air .valve' 11 is 1 closed. TThen the valves in the pipe or pipes 8 at the top of the furnace are opened and gas 'or other hydrocarbon is introduced at the top of the furnace.

The hydrocarbon, passin contact with the very high? downwar decomposed to form hydrogen and carbon black. 7 r

I Theseelements pass outwardly from the base of the furnace through conduit 14, entering the conveying conduit 16, being carried therethi'ough by conveyer 26 through in y heated re ac-v 'tory' surfaces, and in the absence of air, is

the coolin water bath 17, efiectin precipie 'tation of t e carbon, which is disc arged by the conveyer into hopper 21.

The hydrogen gas passing through the automatic pressure regulating valve 46, the

water seal tank 32,,and the washing tanks 34 and 37, and finally to the holder, is, thus completely purities.

The operation above described is contin ued until the,temperature in the furnace, 2

has been reduced to a degree below which entire decomposition; of the hydrocarbon will not occur, whereupon the supply of hydro cleansedof any suspended imcarbon gas through pipe 8 is shut 0d at the top of the furnace, after pressure in the fur.- nace is reduced to atmospheric of the furnace, instead of gas, for the making of hydrogen and carbon black, it may also be sprayed inunder pressure,'or atomized by aid of compressed hydrogen, without air, so that only minute particles of the car tion chamber 9 with an air blast. When the same kind of hydrocarbon is used at'the top Mid bon will strike the hot checkerwork, by using I a suitable atomizer.-

Otherwise the entire checkerwork would soon be clogged with carbon, whereas, when either a gas or very fine spray is-used, the

'finely divided carbon is carried down with the gas.

It will be readily'und rstood that much or ran the carbon will necessarily. adhere to the re fractory material on the inner walls of the furnace, but by observing the above precautions this Wlll be reduced to a Such adhering carbon will be consumed in the next heating operation of the furnace.

Owing to incidental traces of moisture ,in

the hydrocarbon used and possible impuri-- ties such as metallic oxids in the refractory checkerwork, some carbon monoxid is ordinarily produced during the operation of the furnace.

Where the expression absence of metals or metallic oxids is used, it is understood to mean the absence of any supplemental or additional amounts of such, and that any such impurities as remain in the hydrogen are only such small amounts as the hydrocarbon may have added to it, or from the walls of the furnace,-or from the refractory material contained in it.

When it is necessary to remove the carbon monoxid from the gas the apparatus illustrated in Fig. 3 is employed and while the furnace shown in Fig. 1 is being heated up, air and gas is also admitted to the furnace illustrated in Fig. 3. Then when the desired temperature has been obtained in furnace Fig. 1 the gas and air are shut off and gas is admitted at the top of the furnace, the stack valve is closed, and thehydrogen and carbon accumulate in the furnace and in the conveyer and screen box. The automatic valve 46 illustrated in Fig. 3 retains all the gases in these chambers until the desired pressure is obtained.

In case we are running the furnace under a pressure of fifteen pounds above atmospheric pressure a considerable amount of gas will be decomposed before any hydrogen 1 will pass through the regulating valve 46 or 46. a

It may be pointed out that the pressure may be regulated either at the valve 15 between the furnace, Fig. 1, and the conveyer,

or by means of the automatic valve 46 or 46*. When gas begins to pass through the automatic valve 46, steam is admitted into the furnace shown in Fig. 3 and the carbon monoxid in the, gas is oxidized to carbon dioxid by means of the steam in contact with the refractory material or metallic oxids and passes over into the washing tanks Where the carbon dioxid is removed by alkaline materials.

Where suitable natural gas is obtainable,

value, 145 B. T. U. also includes the heat necessary to raise the temperature of the gas to the temperature at which it Wlll be desaid chamber and into contact with the refractory material, and. means for cooling the,

products to separate the carbon from the hydrogen.

3. Apparatus for making carbon black consisting of an inclosing chamber containing highly heated refractory materia1,means for excluding air therefrom, means for introducing a suitable hydrocarbon into said chamber and into contact with the refractory material, and means for cooling the products to separate the carbon from the hydrogen and for subjecting the hydrogen to cleansing operations to eliminate impurities.

4. Apparatus for making carbon black and hydrogen consisting of an inclosing chamber containing highly heated refractory material, means for excluding air there from, means for introducing a suitable hydrocarbon into said chamber and into contact with the refractory material, and means for introducing a combustible fuel into the chamber.

5. Apparatus for making carbon black and hydrogen consisting of an inclosingchamber containing highly heated refractory material, means for excluding air therefrom, means'for introducing a suitable hydrocarbon into said chamber and into contact with the refractory material, means for introducing a combustible fuel into the chamber, and means for cooling the products to separate the carbon from the hydrogen.

6. Apparatus for making carbon black and hydrogen consisting of an inclosing chamber containing highly heated refractory material, means for excluding air therefrom, means for introducing a suitable hydrocarbon into said chamber and into contact withthe refractory material, means for introducing the combustible fuel into the chamber, means for cooling the products to separate the carbon from the hydrogen, and means for subjecting the hydrogen to suitable treatment for the elimination of impurities.

7. Apparatus for making carbon black and hydrogen consisting of an inclosing chamber containing highly heated refractory I modncing a suitable d said ch iaeeoee material, means for excluding air therefrom, means for introducing a suitable hydrocarbon into said chamber and into contact with the refractory material, means for separating the carbon from the hydrogen, means for passing the resulting hydrogen and accompanying carbon monoxid through highly heated refractory material in the presence of steam to oxidize the carbon monoxid, and

means for separating the resulting carbon dioxid.

8. Apparatus for making carbon black and hydrogen consisting of an inclosing chamber containing highly heated refractory material, means for excluding air therefrom, means for introducing a suitable hydrocarbon into said. chamber and into contact with the refractory material, means for separating the carbon from the hydrogen, means for passing the resulting hydrogen and accompanying carbon monoxid through highly heated metallic oxids in the presence of steam to oxidize the carbon monoxid, and means for separating the resulting carbon dioxid.

9. Apparatus for making carbon black and hydrogen consisting of an inclosing chamber containing highly heated refractory material, means for excluding air therefrom, means for introducing a suitable hydrocarbon into said chamber and into contact With the refractory material, means for separating the carbon from the hydrogen, means for passing the resulting hydrogen and accompanying carbon monoxid through highly heated refractory material in the presence of steam to oxidize the carbon monoxid, and means for separating the resulting carbon dioxid.

10. Apparatus for making carbon black and hydrogen consisting of an inclosing chamber containing highly heated refractory material, means for excluding air therefrom, means for introducing a suitable hydrocarbon into said chamber and into con tact with the refractory material, means for separating the carbon from the hydron,

means for passing the resulting hydron and accompanying carbon monoxid through highly heated metallic oxids in the presence of steam to oxidize the carbon monom'd, and means for separating the resulting caon died.

ll. Apparatus for making carbon black ring of an inclg chber contaming highly hted l w i i l e material, mns for excluding air ther om, means for inh mm and into 001mb lulu fractory material, means for atomizing the hydrocarbon in connection with a jet of hydrogen, and means for cooling the products to separate the carbon from the hydrogen.

12. Apparatus for making carbon black and hydrogen comprising a decomposing chamber having a filling of refractory ma terial, means for heating said material, means for introducing hydrocarbon thereto, means for conducting carbon and hydrogen from said decomposing chamber and for cooling the same in transit, and means for collecting precipitated carbon and for carrying off the separated gases.

13. Apparatus for making carbon black and hydrogen comprising a decomposing chamber having a filling of refractory material, means for heating said material, means for introducing hydrocarbon thereto, means for excluding air from said chamber, means for conducting. carbon and hydrogen from said decomposing chamber and for cooling the same in transit, and means for collecting precipitated carbon and for carrying oil the separated gases.

14. Apparatus for making carbon black and hydrogen comprising a decomposing chamber having a fuel combustion chamber, means for introducing fuel thereto, a filling of refractory material Within the chamber, means for introducing hydrocarbon to the chamber and passing it through the heated refractory material, means for excluding air from the chamber during said step, and means for collecting precipitated carbon and for carrying off the separated gases.

15. Apparatus for making carbon black and hydrogen comprising a decomposing chamber having a fuel combustion chamber, means for introducing fuel thereto, a filling of refractory material within the chamber, means for introducing hydrocarbon to the chamber and passing it throu h the heated refractory material, means or excluding air from the chamber during said step, ms for conducting carbon and hydrogen from said decomposing chamber and for cooling the same in transit, and means for collecting precipitated carbon and for cang 0d the separated ses. H

ln testimony whereof we hereunto an our signatures in the presence of o Witc ne: at

nor nno or n. w p

Witnesses:

A. i lit in tin, C. .i i; 

